In my case it depends on the game, since new villagers are added over time and others are forsaken apparently forever. My list would be:
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Animal Crossing (for the Gabe Cube) = Tiara, the snooty rhino. A close second would be Elina, the snooty elephant (islander). Neither of them survived to new installments
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Wild world = definitely Stitches! That hugable lazy cub was introduced in this game.
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City Folk = strangely... Gala, the normal pig. And that's a surprise, because I'm not very fond of pigs (both in-game and real life). But coincidentally she was always so nice to me when I needed someone to the most.
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New Leaf =
Marshal! Since the very first moment. He was the only one I actually cried over when he accidentaly left my town. When I found someone here in the forums willing to give him back to me, I spent all my 700 bells on him. No regrets ever. I wasn't even aware at the time of how popular he actually was, I just loved him on my own. Remains my fave nowadays, nobody can take his place in my heart
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New Horizons = I highly dislike the overall design of this installment, hence why I haven't bougth/played it and have no intention of ever doing so. But from several videos I've watched, I somehow seem to favour Sherb? I've seen him around so much that for a while I was convinced I already knew him from HHD...